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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Simulations of self- and Xe diffusivity in uranium mononitride including chemistry and irradiation effects

A combination of density functional theory and empirical potential atomic scale simulations have been used to determine a model for defect stability and mobility in uranium mononitride (UN), as a function of temperature (T) and N 2 partial pressure (p N 2 ). Using the model, predictions of hypo-stoichiometry under U-rich conditions compare favorably to CALPHAD calculations using the TAF-ID database. Furthermore, our predictions of U and N self-diffusivity are in good agreement with experiments carried out as a function of T at specific partial pressures under thermal equilibrium. The validated atomic scale data have then been implemented within a cluster dynamics method to simulate irradiation-enhanced defect concentrations. All defects and clusters studied have significantly enhanced concentrations, with respect to thermal equilibrium, as T is lowered. The irradiation-enhanced Xe diffusivity is compared to post-irradiation annealing and in-pile experiments. In conclusion, the contributions of various defects and clusters to non-stoichiometry, self-diffusivity, and Xe diffusivity are discussed.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2025

Precise half-life determination of 131 Ba and 125 Xe

Barium-131 and Xenon-125 are valuable radioisotopes with numerous scientific and medical applications. Here, we produced both isotopes via proton irradiation of a cesium iodide (CsI) target at the Brookhaven Tandem Van de Graaff accelerator (BTVG). Following irradiation, we conducted systematic γ-ray spectroscopy measurements at the National Nuclear Data Center (NNDC) decay station using a calibrated High-Purity Germanium (HPGe) detector, collecting data over a 2-month period (spanning approximately 4.5 half-lives for 131 Ba). Through careful analysis of the characteristic γ-ray emissions from both isotopes, we determined the half-life of 131 Ba to be 11.55(6) days, which agrees with the previously evaluated value. For 125 Xe, we measured a half-life of 16.56(8) hours, slightly lower than the evaluated value.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Isotope study of the nonlinear pressure shifts of 85 Rb and 87 Rb hyperfine resonances in Ar, Kr, and Xe buffer gases

Measurements of the 0–0 hyperfine resonant frequencies of ground-state 85 Rb atoms show a nonlinear dependence on the pressure of the buffer gases Ar, Kr, and Xe. The nonlinearities are similar to those previously observed with 87 Rb and 133 Cs and presumed to come from alkali-metal–noble-gas van der Waals molecules. However, the shape of the nonlinearity observed for Xe conflicts with previous theory, and the nonlinearities for Ar and Kr disagree with the expected isotopic scaling of previous 87 Rb results. Improving the modeling alleviates most of these discrepancies by treating rotation quantum mechanically and considering additional spin interactions in the molecules. Including the dipolar-hyperfine interaction allows simultaneous fitting of the linear and nonlinear shifts of both 85 Rb and 87 Rb in either Ar, Kr, or Xe buffer gases with a minimal set of shared, isotope-independent parameters. To the limit of experimental accuracy, the shifts in He and N 2 were linear with pressure. Further, the results are of practical interest to vapor-cell atomic clocks and related devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Fluorescence-mediated postcollision interaction in x-ray photoionization of the Xe 𝐾 edge

Postcollision interaction (PCI) in near-threshold photoionization of the K shell of atomic Xe is investigated with hard-x-ray synchrotron radiation. Applying Auger electron spectroscopy, line-shape distortion is monitored in the K-L 2 → L 2 M 4,5 M 4,5 decay channel, where the initial K-L 2 (Kα 2 ) x-ray-emission step mediates the emission of the two continuum electrons. The K-edge result is compared to similar data obtained on direct L 2 M 4,5 M 4,5 decay at the L 2 edge without x-ray-emission. In conclusion, it is found that the evolution of the PCI shift with excess photon energy is very similar at both edges, but a subtle decrease in the PCI shift is observable at the K edge due to the effect of the ultrafast x-ray emission step delaying the PCI energy exchange by a few attoseconds.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

First direct observation of isomeric decay in neutron-rich odd-odd Ta186

Deexcitation γ rays associated with an isomeric state of 186 Ta were investigated. The isomers were produced in multinucleon transfer reactions between a 136 Xe beam and a natural W target and were collected and separated by the KEK Isotope Separation System. Two γ transitions with energies of 161.1(2) and 186.8(1) keV associated with an isomeric decay were observed for the first time. The half-life of the isomeric state of the neutral atom 186m Ta was deduced as 17(2) s. Based on the comparison with the previous measurements of the isomeric state using the Experimental Storage Ring at GSI Darmstadt and the coupling of angular momenta of individual particle orbitals in odd-odd nuclei, a decay scheme of 186m Ta was proposed.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS1998

Incorporation of Solar Noble Gases from a Nebula-Derived Atmosphere During Magma Ocean Cooling

The presence of solar noble gases in the deep interior of the Earth is inferred from the Ne isotopic compositions of MORB (Mid-ocean Ridge Basalts) and OIB (Oceanic Island Basalt); Ar data may also consistent with a solar component in the deep mantle. Models of the transport and distribution of noble gases in the earth's mantle allow for the presence of solar Ar/Ne and Xe/Ne ratios and permit the calculation of lower mantle noble gas concentrations. These mantle data and models also indicate that the Earth suffered early (0.7 to 2 x 10(exp 8) yr) and large (greater than 99 percent) losses of noble gases from the interior, a result previously concluded for atmospheric Xe. We have pursued the suggestion that solar noble gases were incorporated in the forming Earth from a massive, nebula-derived atmosphere which promoted large-scale melting, so that gases from this atmosphere dissolved in the magma ocean and were mixed downward. Models of a primitive atmosphere captured from the solar nebula and supported by accretion luminosity indicate that pressures at the Earth's surface were adequate (and largely more than the required 100 Atm) to dissolve sufficient gases. We have calculated the coupled evolution of the magma ocean and the overlying atmosphere under conditions corresponding to the cessation (or severe attenuation) of the sustaining accretion luminosity, prior to the complete removal of the solar nebula. Such a condition was likely to obtain, for instance, when most of the unaccumulated mass resided in large bodies which were only sporadically accreted. The luminosity supporting the atmosphere is then that provided by the cooling Earth, consideration of which sets a lower limit to the time required to solidify the mantle and terminate the incorporation of atmospheric gases within it. In our initial calculations, we have fixed the nebula temperature at To = 300K, a value likely to be appropriate for nebular temperatures at lAU in the early planet-building epoch. We treated the background (nebula) pressure as an adjustable, time-dependent parameter. Additional information is contained within the original extended abstract.

Woolum, D. S.↗
NASA NTRS2013

High Current Hollow Cathode Plasma Plume Measurements

Plasma plume measurements are reported for a hollow cathode assembly (HCA) oper-ated at discharge currents of 50, 70, and 100 A at xenon ow rates between 19 - 46 sccm.The HCA was centrally mounted in the annulus of the NASA-300MS Hall Thruster andwas operated in the spot and plume modes with additional data taken with an appliedmagnetic eld. Langmuir probes, retarding potential analyzers, and optical emission spec-troscopy were employed to measure plasma properties near the orice of the HCA and toassess the charge state of the near-eld plasma. Electron temperatures (2-6 eV) and plasmapotentials are consistent with probe-measured values in previous investigations. Operationwith an applied-eld yields higher discharge voltages, increased Xe III production, andincreased signals from the 833.5 nm C I line. While operating in plume mode and with anapplied eld, ion energy distribution measurements yield ions with energies signicantlyexceeding the applied discharge voltage. These ndings are correlated with high-frequencyoscillations associated with each mode.

Plasma diagnostics↗
DOE OSTI2024

Preliminary Analysis of Advanced Reactors Storage, Transportation, and Disposal

Based on the higher interest in Advanced Reactor (AR) deployment (e.g., ARDP[1]) for potential new fuel cycles, the Spent Fuel & Waste Science and Technology (SFWST) Program has begun to evaluate the possible implications of long-term management and final disposition of potential Advance Reactor spent nuclear fuels (SNF) that would be generated in potential advanced reactors. Safely managing and dispositioning the potential future AR SNF, and any other associated radioactive wastes, is the primary focus of this initial preliminary assessment of those. This paper summarizes the efforts by the Spent Fuel & Waste Science and Technology (SFWST) in evaluating characteristics and packaging options for advanced reactor spent nuclear fuel forms. The fuel forms were categorized into three types: (1) tristructural isotropic (TRISO), (2) metallic, and (3) fuel salt. This work emphasized TRISO and metallic SNF and waste streams because of the near-term anticipated operation of the Xe-100 and the Natrium reactors as advanced-reactor demonstrations. Preliminary information for the spent-fuel salts discharged from molten-salt reactors (MSRs) is also examined to provide a baseline for future efforts. All calculations and assumptions used publicly available information. The following characteristics are calculated or estimated for use in the preliminary assessments: SNF volume and mass, radiation/activity levels through time, thermal conditions through time, potential radionuclide source terms, chemical interactions and evolutions, disposal inventories, and waste-form lifetime. Using those characteristics, calculations to determine the applicability of existing canister designs were performed. These evaluations included geometric (e.g., dimension, volume) and mass/weight considerations, known operational approaches and loading procedures, physical and chemical considerations/conditions for storage environments, as-loaded radiation, thermal, and criticality analyses to identify constraints for storage, transportation, and disposal. The paper also includes a literature review and analysis on the storage, transportation, and disposal evaluations and experiences from reactors with similar fuel forms. Advanced-reactor vendors cite past experiences with Fort St. Vrain for TRISO and the Experimental Breeder Reactor II (EBR-II) for metallics that have major influences on fuel design. Finally, the paper includes preliminary concepts of operation for advanced-reactor SNF. This encompasses storage, transportation, potential treatment, and disposal activities from both a per-canister and systems-integration perspective.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS1981

Adsorption of xenon and krypton on shales

A method that uses a mass spectrometer as a manometer is employed in the measurement of Xe and Kr adsorption parameters on shales and related samples, where gas partial pressures were lower than 10 to the -11th atm, corresponding adsorption coverages are only small fractions of a monolayer, and Henry's Law behavior is expected and observed. Results show heats of adsorption in the 2-7 kcal/mol range, and Henry constants at 0-25 C of 1 cu cm STP/g per atmosphere are extrapolated. Although the adsorption properties obtained are variable by sample, the range obtained suggests that shales may be capable of an equilibrium adsorption with modern air high enough to account for a significant fraction of the atmospheric inventory of Xe, and perhaps even of Kr. This effect will nevertheless not account for the factor-of-25 defficiency of atmospheric Xe, in comparison with the planetary gas patterns observed in meteorites.

Podosek, F. A.↗
NASA NTRS1994

Nitrogen and xenon isotopic disequilibrium in Bachmut (L6) chondrule J2689 and matrix

Chondrule J2689, a large (8-mm) RP chondrule from Bachmut (L6) was previously found to be in disequilibrium with its host in a variety of features: (1) It has a fine-grained hornfelsic texture; (2) it contains low amounts of metal with a low-Ni taenite composition not found in the matrix; (3) the Ni/Co ratio of that metal is close to the solar ratio, which is equal to the bulk Ni/Co ratio (23) of the chondrule; (4) the bulk alkali content of the chondrule is high and the Na/K ratio is fractionated with respect to the average L chondrite ratio of 8; (5) Cr is depleted in spite of the high pyroxene content; (6) the siderophile elements are strongly depleted but are fractionated with their abundances increasing with volatility; and (7) the O isotopes of the chondrule and the host are out of equilibrium. However, the (Fe,Mg) silicates, feldspar, and chromite have chemical compositions indistinguishable from that of the host chondrite. We have studied a chip of the chondrite and of adjacent matrix by stepwise heating and by combustion in O for N and Xe isotopic abundances. (1) The chondrule preserved distinct bulk, metal, and O isotopic compositional features. It is therefore unlikely that the 'equilibration' of the major silicates Fe/Mg ratios could have taken place after accretion; (2) the chondrule was well equilibrated before break-up and exposure to cosmic rays; (3) two N signatures in the matrix also indicate that the matrix is not equilibrated; and (4) all data collected so far point toward the presence of unequilibrated Bachmut components. Very few reactions took place after accretion.

Kim, Y.↗
NASA NTRS2014

High Current Hollow Cathode Plasma Plume Measurements

Plasma plume measurements are reported for a hollow cathode assembly (HCA) operated at discharge currents of 50, 70, and 100 A at xenon flow rates between 19 - 46 standard cubic centimeter per minute. The HCA was centrally mounted in the NASA-300MS Hall Thruster and was operated in the "spot" and "plume" modes with additional data taken with an applied magnetic field. Langmuir probes, retarding potential analyzers, and optical emission spectroscopy were employed to measure plasma properties near the orifice of the HCA and to assess the charge state of the near-field plasma. Electron temperatures (2-6 electron volt) and plasma potentials are consistent with probe-measured values in previous investigations. Operation with an applied-field yields higher discharge voltages, increased Xe III production, and increased signals from the 833.5 nm C I line. While operating in plume mode and with an applied field, ion energy distribution measurements yield ions with energies significantly exceeding the applied discharge voltage. These findings are correlated with high-frequency oscillations associated with each mode.

High frequency analysis↗
DOE OSTI2020

Low-diffusion Xe-He gas mixtures for rare-event detection: electroluminescence yield

High pressure xenon Time Projection Chambers (TPC) based on secondary scintillation (electroluminescence) signal amplification are being proposed for rare event detection such as directional dark matter, double electron capture and double beta decay detection. The discrimination of the rare event through the topological signature of primary ionisation trails is a major asset for this type of TPC when compared to single liquid or double-phase TPCs, limited mainly by the high electron diffusion in pure xenon. Helium admixtures with xenon can be an attractive solution to reduce the electron diffusion significantly, improving the discrimination efficiency of these optical TPCs. We have measured the electroluminescence (EL) yield of Xe-He mixtures, in the range of 0 to 30% He and demonstrated the small impact on the EL yield of the addition of helium to pure xenon. For a typical reduced electric field of 2.5 kV/cm/bar in the scintillation region, the EL yield is lowered by ~ 2%, 3%, 6% and 10% for 10%, 15%, 20% and 30% of helium concentration, respectively. This decrease is less than what has been obtained from the most recent simulation framework in the literature. The impact of the addition of helium on EL statistical fluctuations is negligible, within the experimental uncertainties. The present results are an important benchmark for the simulation tools to be applied to future optical TPCs based on Xe-He mixtures.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

Fluorescence imaging of individual ions and molecules in pressurized noble gases for barium tagging in 136Xe

Abstract The imaging of individual Ba 2+ ions in high pressure xenon gas is one possible way to attain background-free sensitivity to neutrinoless double beta decay and hence establish the Majorana nature of the neutrino. In this paper we demonstrate selective single Ba 2+ ion imaging inside a high-pressure xenon gas environment. Ba 2+ ions chelated with molecular chemosensors are resolved at the gas-solid interface using a diffraction-limited imaging system with scan area of 1 × 1 cm 2 located inside 10 bar of xenon gas. This form of microscopy represents key ingredient in the development of barium tagging for neutrinoless double beta decay searches in 136 Xe. This also provides a new tool for studying the photophysics of fluorescent molecules and chemosensors at the solid-gas interface to enable bottom-up design of catalysts and sensors.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2022

Cross-polarized common-path temporal interferometry for high-sensitivity strong-field ionization measurements

Absolute density measurements of low-ionization-degree or low-density plasmas ionized by lasers are very important for understanding strong-field physics, atmospheric propagation of intense laser pulses, Lidar etc. A cross-polarized common-path temporal interferometer using balanced detection was developed for measuring plasma density with a sensitivity of ∼0.6 mrad, equivalent to a plasma density-length product of ∼2.6 × 10 13 cm −2 if using an 800 nm probe laser. By using this interferometer, we have investigated strong-field ionization yield versus intensity for various noble gases (Ar, Kr, and Xe) using 800 nm, 55 fs laser pulses with both linear (LP) and circular (CP) polarization. The experimental results were compared to the theoretical models of Ammosov-Delone-Krainov (ADK) and Perelomov-Popov-Terent’ev (PPT). We find that the measured phase change induced by plasma formation can be explained by the ADK theory in the adiabatic tunneling ionization regime, while PPT model can be applied to all different regimes. We have also measured the photoionization and fractional photodissociation of molecular (MO) hydrogen. By comparing our experimental results with PPT and MO-PPT models, we have determined the likely ionization pathways when using three different pump laser wavelengths of 800 nm, 400 nm, and 267 nm.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Iodine Sorption on AgZ-PAN

The Department of Energy (DOE) Nuclear Fuel Cycle and Supply Chain Program Material Recovery and Waste Form Development (MRWFD) Campaign Off-gas Sigma Team has performed research and development on iodine control and iodine waste forms for the past several years. This research and development has included iodine adsorption tests using a laboratory-scale test system containing multiple-segmented fixed beds of iodine adsorbents. Iodine capture performance has been tested using (a) non-radioactive synthetic gas mixtures blended from air, nitrogen, NO, NO 2 , water, to simulate dissolver off-gas (DOG) and vessel off-gas (VOG) streams from used nuclear fuel aqueous reprocessing, (b) inorganic and organic iodine species, and (c) different sorbents. An initial test of silver-functionalized mordenite in polyacrylonitrile matrix (AgZ-PAN) was conducted to assess if this sorbent, initially designed for selective sorption of Xe that evolves into used fuel reprocessing off-gas streams, could also be a candidate for iodine sorption. This test was conducted using the same deep-bed test system and methodologies used in many prior iodine sorption tests using other sorbents. Diatomic iodine (I2) was used as the target iodide in a gas stream containing air, NO, NO 2 , and moisture designed to simulate an aqueous reprocessing dissolver off-gas (DOG) stream.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
NASA NTRS1980

Isotopic anomalies of noble gases in meteorites and their origins. VI Presolar components in the Murchison C2 chondrite

Rare gases were analyzed by stepped heating in five fractions of a chemically resistant residue from Murchison that had been separated according to grain size and resistance to HClO4. Nine gas components were recognized, of which three appear to be presolar: (1) Ne-E(H) released at 1000-1600 C and located in spinel; (2) Ne-E(L) released at less than 800 C and apparently located in a carbonaceous phase of grain size up to 10 microns; and (3) s-process Xe and Kr released at 1200-1600 C and located in a poorly characterized, possibly carbonaceous phase, distinct from the host phase of Ne-E(L).

Alaerts, L.↗
DOE OSTI2023

Spectroscopic quadrupole moments in 124 $\mathrm{Xe}$

The Xe isotopic chain with four valence protons above the Z=50 shell closure is an ideal laboratory for the study of the evolution of nuclear deformation. At the N=82 shell closure, 136 Xe presents all characteristics of a doubly closed shell nucleus with a spherical shape. In the very neutron-deficient isotopes close to N=50, the α-decay chain of Xe was investigated to probe the radioactive decay properties near the drip-line and the magicity of 100 Sn. Additionally, the Xe isotopes present higher order symmetries in the nuclear deformation such as the octupole degree of freedom near N=60 and N=90 or O(6) symmetry in stable isotopes. The relevance of the O(6) symmetry has been investigated by measuring the spectroscopic quadrupole moment of the first excited states in 124 Xe. In the O(6) symmetry limit, the spectroscopic quadrupole moment of collective states is expected to be null. A stable 124 Xe beam with energies of 4.03A MeV and 4.11 A MeV was used to bombard a nat W target at the GANIL facility. Excited states were populated via the safe Coulomb excitation reaction. The collision of the heavy ions with a large Z at low energy make this reaction sensitive to the diagonal E2 matrix element of the excited states. The recoils were detected in the VAMOS++ magnetic spectrometer and the γ rays in the AGATA tracking array. The least squares fitting code gosia was used for the analysis to extract both E2 and M1 transitional and E2 diagonal matrix elements. The rotational ground state band was populated up to the 8$^{+}_{1}$ state as well as the 2$^{+}_{2}$ and 4$^{+}_{2}$ states. Using high precision spectroscopic data to constrain the gosia fit, the spectroscopic quadrupole moments of the 2$^{+}_{1}$, 4$^{+}_{1}$, and 6$^{+}_{1}$ states were determined for the first time. The spectroscopic quadrupole moments were found to be negative, large, and constant in the ground state band underlining the prolate axially deformed ground state band of 124 Xe. Here, the present experimental data confirm that the O(6) symmetry is substantially broken in 124 Xe .

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS1980

Lunar and Planetary Science Conference, 11th, Houston, TX, March 17-21, 1980, Proceedings. Volume 2 - Meteorite and regolith studies

Topics discussed include studies of chondrites, mesosiderites, and achondrites; isotope modeling; Antarctic weathering; irradiation effects; lunar regolith studies; the Apollo 17 drill core; soils and agglutinates; and volatiles. Particular attention is given to the proportional retention of I and Xe-129 in preheated Allende, olivine clasts from mesosiderites and howardites as clues to the nature of achondritic parent bodies, a record of solar corpuscular radiation in minerals from lunar soils, the experimental shock metamorphism of lunar soil, and the clouding of pyroxene and plagioclase in eucrites.

Merrill, R. B.↗